WO2012156639A1 - Metal-air accumulator with air electrode protection device - Google Patents
Metal-air accumulator with air electrode protection device Download PDFInfo
- Publication number
- WO2012156639A1 WO2012156639A1 PCT/FR2012/051080 FR2012051080W WO2012156639A1 WO 2012156639 A1 WO2012156639 A1 WO 2012156639A1 FR 2012051080 W FR2012051080 W FR 2012051080W WO 2012156639 A1 WO2012156639 A1 WO 2012156639A1
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- WO
- WIPO (PCT)
- Prior art keywords
- electrode
- terminal
- air
- positive electrode
- switching
- Prior art date
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Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
- H01M10/425—Structural combination with electronic components, e.g. electronic circuits integrated to the outside of the casing
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
- H01M10/44—Methods for charging or discharging
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
- H01M10/48—Accumulators combined with arrangements for measuring, testing or indicating the condition of cells, e.g. the level or density of the electrolyte
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M12/00—Hybrid cells; Manufacture thereof
- H01M12/08—Hybrid cells; Manufacture thereof composed of a half-cell of a fuel-cell type and a half-cell of the secondary-cell type
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/50—Current conducting connections for cells or batteries
- H01M50/572—Means for preventing undesired use or discharge
- H01M50/574—Devices or arrangements for the interruption of current
-
- H—ELECTRICITY
- H02—GENERATION; CONVERSION OR DISTRIBUTION OF ELECTRIC POWER
- H02J—CIRCUIT ARRANGEMENTS OR SYSTEMS FOR SUPPLYING OR DISTRIBUTING ELECTRIC POWER; SYSTEMS FOR STORING ELECTRIC ENERGY
- H02J7/00—Circuit arrangements for charging or depolarising batteries or for supplying loads from batteries
- H02J7/0068—Battery or charger load switching, e.g. concurrent charging and load supply
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Definitions
- the present invention relates to a rechargeable metal-air accumulator comprising an air electrode, an oxygen-releasing electrode and an automatic device for protecting the air electrode during charging and discharging of the accumulator.
- the invention also relates to a method for storing and restoring electrical energy using such an accumulator.
- Metal-air batteries use a negative electrode based on a metal such as zinc, iron or lithium, coupled to an air electrode.
- a metal such as zinc, iron or lithium
- molecular oxygen is reduced to the positive electrode and the metal is oxidized to the negative electrode:
- the two electrodes are most often in contact with an aqueous alkaline electrolyte.
- Zinc air batteries are marketed for example for use in hearing aids.
- Air electrodes have the advantage of being able to use oxygen as an oxidizing agent for electrochemical reduction, available in unlimited quantities anywhere and at any time. A large reaction surface is however necessary because the density of oxygen in the air is low (0.03 mol / L).
- the porous solid structure of the air electrodes provides this high reaction surface.
- An air electrode is a porous solid structure in contact with a liquid electrolyte, generally an alkaline aqueous solution.
- the interface between the air electrode and the liquid electrolyte is a "triple contact" interface in which the active material of the electrode, the gaseous oxidant and the liquid electrolyte are simultaneously present.
- the air electrodes have a considerable disadvantage, which is their great fragility when they are used during recharging of the accumulator.
- the air electrode has a porous structure and functions as a voluminal electrode in which the electrochemical reaction takes place in the entire volume of the electrode, at the interface between the gaseous oxidant and the liquid electrolyte. and the solid active ingredient (triple contact).
- molecular oxygen gas is formed within the structure of the air electrode. This gaseous oxygen quickly results in the mechanical destruction of the porous structure of the air electrode by breaking the bonds between the carbon grains and the binder polymer used.
- the inventors have also observed that the oxygen reduction catalysts incorporated in the air electrode at the surface of the carbon grains are not stable at the high potentials necessary for the reverse oxidation reaction. Some authors have used more resistant oxygen reduction catalysts coupled to an oxygen evolution catalyst in a bifunctional electrode composed of two electrically coupled layers (see US 5,306,579). This configuration, however, produces electrodes having a low life and a limited number of cycles.
- the object of the present invention is to provide effective protection of the porous air electrode of a metal-air accumulator not only during the charging phase of the accumulator, but also during discharge.
- the subject of the present invention is therefore a rechargeable accumulator comprising one or more metal-air cells, each cell comprising
- a negative metal electrode for a metal-air cell connected to the first terminal
- a second positive electrode which is a porous air electrode containing at least one oxygen reduction catalyst
- control means adapted to continuously compare the measured voltage (V m ) between the second terminal and the first terminal to a reference value (V c ) and to send a switching signal to the switching means when the measured voltage ( V m ) becomes smaller than the set value (V c ),
- switching means adapted to receive a switching signal from the control means and to connect and disconnect the air electrode of the second terminal.
- the accumulator of the present invention thus comprises, in each of its cells, three types of electrodes:
- a first positive electrode which, in one embodiment, is continuously connected to the second terminal or which, in another embodiment, is connected to the second terminal alternately with the second positive electrode, i.e. say it is disconnected from the second terminal at the time of the connection of the second positive electrode and
- an air electrode (second positive electrode) which is to be protected against degradation and which is connected to the second terminal only during the second discharge phase when the potential between the two terminals is sufficiently low.
- the present invention also encompasses variants where one or more of these electrodes is present in multiple or multiple parts.
- a cell with a single negative electrode in the form of a plate, two air electrodes located on one side and the other of the negative electrode and two positive metal electrodes (release electrodes of oxygen) located between the plate-shaped negative electrode and the two air electrodes.
- the negative electrode may in principle be any metal electrode commonly used in a metal-air cell. It may be for example an iron, lithium or zinc electrode, preferably a lithium electrode (Li / LiOH) or a zinc electrode (Zn / Zn (OH) 4 ), and particularly preferably a zinc electrode.
- the first positive oxygen evolution electrode may be, for example, a silver electrode (Ag / AgO) or a nickel electrode (Ni / NiO or NIOH / NiOOH).
- this electrode preferably a nickel electrode, typically has a grid or perforated plate type structure, and is generally located between the negative electrode and the air electrode.
- the perforated structure of this electrode serves, in known manner, to ensure the free passage of the constituents of the liquid electrolyte between the negative electrode and the air electrode during the discharge.
- the second positive electrode is a porous air electrode designed to allow triple contact between the electrolyte, the gaseous oxidant and the solid active material of the electrode. It can be chosen in principle from all those usually used in the art and described in particular in the article by Neburchilov mentioned above.
- the specific surface of the carbon can be increased by reaction with a gas such as CO 2 , prior to its incorporation into the air electrode.
- the high specific surface area of the carbon grains is crucial. Indeed, the more important it is, the higher the current density per unit of geometric electrode surface is high.
- the porous electrode is manufactured by agglomeration of the carbon grains using a binder which is preferably a fluorinated hydrophobic polymer such as FEP sold by the company Dupont.
- a binder which is preferably a fluorinated hydrophobic polymer such as FEP sold by the company Dupont.
- the air electrode based on carbon particles, preferably further contains at least one oxygen reduction catalyst.
- This oxygen reduction catalyst is preferably selected from the group consisting of manganese oxide and cobalt oxide. These catalysts, although very effective, are however deactivated when they are subjected to too high potentials and the automatic protection device of the present invention, formed by the combination of a control means and a switching means, described in more detail below, is therefore particularly important when using these oxygen reduction catalysts.
- the electrolyte used is preferably an aqueous alkaline electrolyte in contact with all the electrodes of the cell.
- a lithium electrode is used as a negative electrode, it may be necessary to physically and in known manner separate the aqueous electrolyte from the negative electrode by a solid electrolyte conducting lithium ions.
- the control means used in the present invention must be adapted to continuously compare the measured voltage (V m ) between the second terminal and the first terminal to a set value (V c ).
- This reference value is for example the value of a reference voltage supplied by a stabilized voltage source powered by the battery or by an external battery. It is preferably set at a value slightly lower than the open circuit cell voltage in the charged state when only the air electrode is connected, ie about 1.44V for a zinc air battery and 3V for a lithium-ion battery. air.
- An electromechanical relay controlled by an operational amplifier is preferably used as control means.
- Such an operational amplifier is marketed for example by the National Semiconductor company under the reference LM324, and will be described in more detail with reference to FIG. 2.
- the present invention also relates to a method of storing and restoring electrical energy using an accumulator as described above.
- This process comprises the following successive steps:
- the Applicant considers that the succession of steps (b) and (c), that is to say the non connection of the air electrode at the beginning of discharge, the continuous monitoring of the decrease of the voltage between the two terminals by appropriate control means, and then the connection of the air electrode only when the absolute value of the potential difference between the terminals has become sufficiently low, allows effective protection of the air electrode and constitutes the contribution of the present invention in the state of the art.
- the voltage at the start of charging is typically equal to 1.7 V.
- the control device When the value of the voltage between the two terminals, measured continuously by the control means, becomes smaller than the set value (1.44 V), the control device sends a switching signal to the switching means in order to finally connect the air electrode to the second terminal.
- the air electrode can remain connected until the end of the discharge step, that is to say until the beginning of the next charging phase.
- the disconnection (step (e)) of the air electrode before the next charge (step (a)) can be done manually or, preferably, automatically through the control means associated with the switching means performing the first switching step (step (c)) of the process according to the invention.
- the first positive electrode can be connected or disconnected.
- This connection or disconnection depends on the structure of the switching means.
- the switching means is adapted to disconnect the first positive electrode from the second terminal.
- the switching means is adapted not to disconnect the first positive electrode from the second terminal, which therefore remains connected continuously to the second terminal, both in charge and discharge.
- Figure 1 is a schematic representation of an embodiment of a cell of an accumulator of the present invention
- FIG. 2 is a schematic representation of control means and switch means forming the air electrode protection device of the present invention.
- the cell of the accumulator has a first terminal 1 and a second terminal 2.
- the first terminal is a negative terminal and the second terminal is a positive terminal.
- the first terminal 1 is connected to a first metal electrode 3, called negative electrode, for example zinc or lithium.
- the second terminal 2 is coupled, via a switching means 7, to an oxygen releasing electrode 4 or to an air electrode 5.
- these two electrodes form positive electrodes .
- the oxygen release electrode may be, for example, nickel.
- the air electrode is a porous carbon-based electrode having at the solid / gas interface a catalyst for reducing oxygen.
- the catalyst may be manganese oxide or cobalt oxide.
- the three electrodes 3, 4, 5 are in contact with at least one electrolyte, preferably an aqueous alkaline liquid electrolyte.
- the two positive electrodes 4, 5 are coupled to the second terminal 2 via switching means 7.
- the switching means 7 are exclusive, that is to say that they connect the terminal 2 either to the oxygen release electrode 4 or to the air electrode 5.
- the accumulator according to the invention further comprises control means 6, adapted to continuously measure the voltage V m between the two terminals 1 and 2 and to send a switching signal to the switching means 7 and thus to control the connection or the disconnection of one and / or the other positive electrode.
- the control means are shown in greater detail in FIG.
- a reference voltage equal to the nominal voltage (V c ) is provided by a stabilized voltage source 8 connected between the first terminal 1 and a negative input of an operational amplifier 9.
- the second terminal 2 is connected to a positive input of the operational amplifier 9 which measures a difference in voltage between the two inputs.
- the setpoint voltage is subtracted from the voltage between the first terminal and the second terminal.
- the amplifier measures a zero difference between the voltages applied to its two inputs.
- the control means 6 furthermore comprise a transistor 10 acting as a switch on a current loop between two terminals 11 and 12.
- the operational amplifier sends a given voltage to the base B of the transistor 10.
- the transistor 10 then becomes conductive and leaves pass a current between its emitter E and its collector C.
- the control means further comprise a coil, or an inductor, 13. When the current flows in the current loop, the coil emits a magnetic field.
- the switching means 7 may comprise a relay comprising a conductive element 14 displaceable under the influence of a magnetic field.
- the conductive element 14 is moved from a first position to a second position. In the first position, the conductive element is moved away from the air electrode so as to disconnect it from the second terminal of the accumulator and in the second position the air electrode is connected to the second terminal of the accumulator. .
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- Engineering & Computer Science (AREA)
- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Manufacturing & Machinery (AREA)
- Microelectronics & Electronic Packaging (AREA)
- Power Engineering (AREA)
- Hybrid Cells (AREA)
- Inert Electrodes (AREA)
- Secondary Cells (AREA)
Abstract
Description
Claims
Priority Applications (9)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
EP12728689.6A EP2710663B1 (en) | 2011-05-19 | 2012-05-15 | Metal-air accumulator with air electrode protection device |
KR1020137033740A KR101664289B1 (en) | 2011-05-19 | 2012-05-15 | Metal-air accumulator with air electrode protection device |
SG2013085147A SG195019A1 (en) | 2011-05-19 | 2012-05-15 | Metal-air accumulator with air electrode protection device |
JP2014510861A JP6198720B2 (en) | 2011-05-19 | 2012-05-15 | Metal-air storage battery with air electrode protection device |
CN201280024018.4A CN103650232B (en) | 2011-05-19 | 2012-05-15 | There is the air-metal batteries of air electrode protection device |
KR1020167002861A KR101674628B1 (en) | 2011-05-19 | 2012-05-15 | Metal-air accumulator with air electrode protection device |
ES12728689.6T ES2546604T3 (en) | 2011-05-19 | 2012-05-15 | Metal-air battery with an air electrode protection device |
US14/117,527 US9293757B2 (en) | 2011-05-19 | 2012-05-15 | Metal-air accumulator with air electrode protection device |
DK12728689.6T DK2710663T3 (en) | 2011-05-19 | 2012-05-15 | METAL AIR ACCUMULATOR WITH AIR ELECTRODE PROTECTION DEVICE |
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
FR1154356A FR2975534B1 (en) | 2011-05-19 | 2011-05-19 | METAL-AIR ACCUMULATOR WITH PROTECTION DEVICE FOR THE AIR ELECTRODE |
FR1154356 | 2011-05-19 |
Publications (1)
Publication Number | Publication Date |
---|---|
WO2012156639A1 true WO2012156639A1 (en) | 2012-11-22 |
Family
ID=46321114
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
PCT/FR2012/051080 WO2012156639A1 (en) | 2011-05-19 | 2012-05-15 | Metal-air accumulator with air electrode protection device |
Country Status (11)
Country | Link |
---|---|
US (1) | US9293757B2 (en) |
EP (1) | EP2710663B1 (en) |
JP (2) | JP6198720B2 (en) |
KR (2) | KR101674628B1 (en) |
CN (2) | CN103650232B (en) |
DK (1) | DK2710663T3 (en) |
ES (1) | ES2546604T3 (en) |
FR (1) | FR2975534B1 (en) |
PT (1) | PT2710663E (en) |
SG (1) | SG195019A1 (en) |
WO (1) | WO2012156639A1 (en) |
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Also Published As
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CN105514517B (en) | 2019-01-11 |
KR20160021894A (en) | 2016-02-26 |
JP6198720B2 (en) | 2017-09-20 |
US20140191727A1 (en) | 2014-07-10 |
JP6200978B2 (en) | 2017-09-20 |
KR20140027410A (en) | 2014-03-06 |
DK2710663T3 (en) | 2015-09-07 |
FR2975534A1 (en) | 2012-11-23 |
JP2014519681A (en) | 2014-08-14 |
CN103650232B (en) | 2016-10-26 |
CN103650232A (en) | 2014-03-19 |
EP2710663B1 (en) | 2015-06-10 |
US9293757B2 (en) | 2016-03-22 |
JP2016136521A (en) | 2016-07-28 |
KR101664289B1 (en) | 2016-10-11 |
CN105514517A (en) | 2016-04-20 |
EP2710663A1 (en) | 2014-03-26 |
ES2546604T3 (en) | 2015-09-25 |
FR2975534B1 (en) | 2013-06-28 |
PT2710663E (en) | 2015-10-08 |
KR101674628B1 (en) | 2016-11-09 |
SG195019A1 (en) | 2013-12-30 |
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